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Post-training quantization (PTQ) is an effective technique for compressing large language models (LLMs). However, while uniform-precision quantization is computationally efficient, it often compromises model performance. To address this, we propose SliM-LLM, a salience-driven mixed-precision quantization framework that allocates bit-widths at the group-wise with high accuracy. Our approach leverages the observation that important weights follow a structured distribution and introduces two key components: 1) Salience-Determined Bit Allocation adaptively assigns bit-widths to groups within each layer based on their salience; and 2) Salience-Weighted Quantizer Calibration optimizes quantizer parameters by incorporating element-level salience, retain essential information. With its structured group-wise partitioning, SliM-LLM provides a hardware-friendly solution that matches the efficiency of uniform quantization methods while significantly improving accuracy. Experiments show that SliM-LLM achieves superior performance across various LLMs at low bit-widths. For example, a 2-bit quantized LLaMA-7B model reduces memory usage by nearly 6x compared to the floating-point baseline, decreases perplexity by 48% compared to state-of-the-art gradient-free PTQ methods, and maintains GPU inference speed. Additionally, the extended version, SliM-LLM+, which incorporates gradient-based quantization, further reduces perplexity by 35.1%. Our code isavailable at https://github.com/Aaronhuang-778/SliM-LLM.